The implementation of carbon capture and storage process (CCS) has been unsuccessful to date, mainly due to the technical issues and high costs associated with two main stages: (1) CO separation from flue gas and (2) CO injection in deep geological deposits, more than 300 m, where CO is in supercritical conditions. This study proposes, for the first time, an enhanced CCS process (e-CCS), in which the stage of CO separation is removed and the flue gas is injected directly in shallow reservoirs located at less than 300 m, where the adsorptive phenomena control CO storage. Nitrogen-rich carbon nanospheres were used as modifying agents of the reservoir porous texture to improve both the CO adsorption capacity and selectivity. For this purpose, sandstone was impregnated with a nanofluid and CO adsorption was evaluated at different pressures (atmospheric pressure and from 3 × 10 MPa to 3.0 MPa) and temperatures (0, 25, and 50 °C). As a main result, a mass fraction of only 20% of nanomaterials increased both the surface area and the molecular interactions, so that the increase of adsorption capacity at shallow reservoir conditions (50 °C and 3.0 MPa) was more than 677 times (from 0.00125 to 0.9 mmol g).